核动力工程2024,Vol.45Issue(6) :121-131.DOI:10.13832/j.jnpe.2024.06.0121

铀电解精炼过程中浓差极化及电极动力学的模拟研究

Simulation Study on Concentration Polarization and Electrode Kinetics during Electrorefining of Uranium

梁柏 张萌 孙兰昕 王靖阳 林如山 韩伟 矫彩山
核动力工程2024,Vol.45Issue(6) :121-131.DOI:10.13832/j.jnpe.2024.06.0121

铀电解精炼过程中浓差极化及电极动力学的模拟研究

Simulation Study on Concentration Polarization and Electrode Kinetics during Electrorefining of Uranium

梁柏 1张萌 1孙兰昕 1王靖阳 1林如山 2韩伟 3矫彩山1
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作者信息

  • 1. 哈尔滨工程大学核安全与仿真技术国防重点学科实验室,哈尔滨,150001
  • 2. 中国原子能科学研究院放射化学研究所,北京,102413
  • 3. 哈尔滨工程大学材料科学与化学工程学院,哈尔滨,150001
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摘要

通过Nernst方程将浓度与过电位相关联,构建了浓度依赖的Butler-Volmer电极动力学公式.基于支持电解质理论优化了传质方程和电位分布方程,改进了铀电解精炼模型.利用新模型分别模拟了循环伏安曲线、恒电位沉积过程和恒电流沉积过程,定量分析了不同电解条件下的浓差极化现象和电极动力学行为.模拟循环伏安曲线与实验结果吻合较好,验证了模型的准确性.通过模拟得到了U(III)浓度、电位和电流密度等在熔盐中和电极表面的分布,预测了扩散层厚度、极限扩散电流和沉积层厚度等关键参数,对比了恒电流沉积和恒电位沉积过程中浓差极化引起的驱动力变化.本研究建立的数值模型可作为优化工艺参数和设计工艺设备的有力工具,对深化理解铀电解精炼机理具有重要物理意义.

Abstract

A concentration-dependent Butler-Volmer electrode kinetics equation was established by correlating concentration with the overpotential through the Nernst equation.The mass transfer equation and potential distribution equation were optimized based on the supporting electrolyte theory,and the uranium electrorefining model was improved.The cyclic voltammetry curve,constant potential deposition process and constant current deposition process were simulated by using the new model,and the concentration polarization phenomenon and electrode dynamic behavior under different electrolytic conditions were quantitatively analyzed.The simulated cyclic voltammetry curve is in good agreement with the experimental results,verifying the accuracy of the model.Through modeling,the distributions of U(III)concentration,potential,and current density in the molten salt and on the surface of electrode were obtained.The key parameters such as diffusion layer thickness,limiting diffusion current and deposition layer thickness were predicted,and the driving force changes caused by concentration polarization during constant current deposition and constant potential deposition were compared.The numerical model established in this study can be used as a powerful tool to optimize process parameters and design process equipment,and has important physical significance for deepening understanding of uranium electrorefining mechanism.

关键词

/电解精炼/浓差极化/电极动力学/数值模拟

Key words

Uranium/Electrorefining/Concentration polarization/Electrode kineticss/Numerical simulation

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出版年

2024
核动力工程
中国核动力研究设计院

核动力工程

CSTPCD北大核心
影响因子:0.3
ISSN:0258-0926
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